Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres

This report details the continued investigation of process variables involved in converting sol-gel-derived, urania-carbon microspheres to ∼820-μm-dia. UC1-xNx fuel kernels in flow-through, vertical Mo and W crucibles at temperatures up to 2123 K. Experiments included calcining of air-dried UO3-H2O-C microspheres in Ar and H2-containing gases, conversion of the resulting UO2-C kernels to dense UO2:2UC in the same gases and vacuum, and its conversion in N2 to UC1-xNx (x = ∼0.85). The thermodynamics of the relevant reactions were applied extensively to interpret and control the process variables. Producing the precursor UO2:2UC kernel of ∼96% theoretical density was required, but its subsequent conversion to UC1-xNx at 2123 K was not accompanied by sintering and resulted in ∼83-86% of theoretical density. Increasing the UC1-xNx kernel nitride component to ∼0.98 in flowing N2-H2 mixtures to evolve HCN was shown to be quantitatively consistent with present and past experiments and the only useful application of H2 in the entire process.